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A low-cost and indium-tin-oxide (ITO)-free electrode-based flexible perovskite solar cell (PSC) that can be fabricated by roll-to-roll processing shall be developed for successful commercialization. High processing temperatures present a challenge for the PSC fabrication on flexible substrates. The most efficient planar n-i-p PSC structures, which utilize a metal oxide as an electron transport layer (ETL), necessitate high annealing temperatures. In addition, the device performance deteriorates owing to the migration of halogen ions, which causes the oxidation of the metal electrodes. These drawbacks conflict with the development of highly efficient flexible PSCs fabricated on ITO-free transparent electrodes. Herein, an efficient ETL material that enables low-temperature processing is presented. Tin dioxide (SnO2) is modified by (sulfobetaine-N,N-dimethylamino)propyl naphthalene diimide (NDI-B) and used as an ETL. The NDI-B effectively reduces the interfacial nonradiative recombination between the ETL and perovskite and suppresses the ion migration by passivating oxygen-vacancy defects in SnO2 and strongly interacting with halogen ions, respectively. Based on the NDI-B-blended SnO2 ETL, a record PCE of 17.48% is achieved in the ITO-free flexible PSC fabricated at low temperature.
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The temperature-dependent evolution of the Kondo lattice is a long-standing topic of theoretical and experimental investigation and yet it lacks a truly microscopic description of the relation of the basic f-c hybridization processes to the fundamental temperature scales of Kondo screening and Fermi-liquid lattice coherence. Here, the temperature dependence of f-c hybridized band dispersions and Fermi-energy f spectral weight in the Kondo lattice system CeCoIn5 is investigated using f-resonant angle-resolved photoemission spectroscopy (ARPES) with sufficient detail to allow direct comparison to first-principles dynamical mean-field theory (DMFT) calculations containing full realism of crystalline electric-field states. The ARPES results, for two orthogonal (001) and (100) cleaved surfaces and three different f-c hybridization configurations, with additional microscopic insight provided by DMFT, reveal f participation in the Fermi surface at temperatures much higher than the lattice coherence temperature, [Formula: see text] K, commonly believed to be the onset for such behavior. The DMFT results show the role of crystalline electric-field (CEF) splittings in this behavior and a T-dependent CEF degeneracy crossover below [Formula: see text] is specifically highlighted. A recent ARPES report of low T Luttinger theorem failure for CeCoIn5 is shown to be unjustified by current ARPES data and is not found in the theory.
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Direct arylation polymerization (DArP) is a synthetic method for conjugated polymers; in DArP, organometallic functionalization steps are omitted and there are no toxic byproducts. As a result, it is considered a more sustainable alternative compared to conventional methods such as Stille polymerization. To explore the possibility of DArP-based polymers as donor materials in organic solar cells (OSCs), a series of conjugated polymers based on the structure of PDCBT (poly[2,2''''-bis[[(2-butyloctyl)oxy]carbonyl][2,2':5',2'':5'',2'''-quaterthiophene]-5,5'''-diyl]) are synthesized using DArP and Stille polymerization. By controlling the monomer concentration and reaction time in DArP, DArP-5 with the highest Mn (21.9 kDa) can be obtained and its optoelectronic properties, electrochemical properties, and microscopic molecular ordering are comparable to those of Stille-based PDCBT (Stille-P). Analysis of the polymer structure indicates no structural defects such as crosslinking from undesired ß-coupling reactions in DArP-5. Upon blending with the PC71 BM acceptor molecule, an increase in the crystallite size of DArP-5 is also observed. In OSC devices with a polymer:PC71 BM bulk-heterojunction photoactive layer, DArP-5 demonstrates a comparable power conversion efficiency of 5.8% with that of Stille-P (5.5%). These results prove that DArP is suitable for synthesizing PDCBT, and DArP-based PDCBT can be used in OSCs as an alternative of Stille-based one.
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Effective exploration is one of the critical factors affecting performance in deep reinforcement learning. Agents acquire data to learn the optimal policy through exploration, and if it is not guaranteed, the data quality deteriorates, which leads to performance degradation. This study investigates the effect of initial entropy, which significantly influences exploration, especially in the early learning stage. The results of this study on tasks with discrete action space show that (1) low initial entropy increases the probability of learning failure, (2) the distributions of initial entropy for various tasks are biased towards low values that inhibit exploration, and (3) the initial entropy for discrete action space varies with both the initial weight and task, making it hard to control. We then devise a simple yet powerful learning strategy to deal with these limitations, namely, entropy-aware model initialization. The proposed algorithm aims to provide a model with high initial entropy to a deep reinforcement learning algorithm for effective exploration. Our experiments showed that the devised learning strategy significantly reduces learning failures and enhances performance, stability, and learning speed.
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Algoritmos , Reforço Psicológico , Conscientização , Entropia , ProbabilidadeRESUMO
Herein, we design and characterize 9-heterocyclic ring non-fullerene acceptors (NFAs) with the extended backbone of indacenodithiophene by cyclopenta [2,1-b:3,4-b'] dithiophene (CPDT). The planar conjugated CPDT donor enhances absorption by reducing vibronic transition and charge transport. Developed NFAs with different end groups shows maximum absorption at approximately 790-850 nm in film. Because of the electronegative nature of the end-group, the corresponding acceptors showed deeper LUMO energy levels and red-shifted ultraviolet absorption. We investigate the crystallinity, film morphology, surface energy, and electronic as well as photovoltaic performance. The organic photovoltaic cells using novel NFAs with the halogen end groups fluorine or chlorine demonstrate better charge collection and faster exciton dissociation than photovoltaic cells using NFAs with methyl or lacking a substituent. Photovoltaic devices constructed from m-Me-ITIC with various end groups deliver power conversion efficiencies of 3.6-11.8%.
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BACKGROUND: Exclusive enteral nutrition (EEN) induces remission in pediatric Crohn's disease (CD). The exact mechanism of EEN therapy in CD is unknown, but alteration of the intestinal microflora after EEN is thought to affect mucosal healing. To determine the link between EEN therapy and therapeutic efficacy in CD, we established a murine model of dextran sulfate sodium (DSS)-induced colitis and applied EEN therapy. METHODS: Eight-week-old C57BL/6 mice were administered DSS for 4 days to induce colitis, and either normal chow (NC) or EEN was administered for the following 4 days. The mice were grouped according to the feeding pattern after DSS administration: DSS/NC and DSS/EEN groups. The clinical course was confirmed via daily observation of the weight and stool. Fecal samples were collected and 16sRNA sequencing was used. The mice were sacrificed to confirm colonic histopathology. RESULTS: Weight reduction and increase in disease activity were observed as the day progressed for 4 days after DSS administration. There was significant weight recovery and improvement in disease activity in the EEN group compared to that in the NC group. Verrucomicrobia and Proteobacteria abundances tended to increase and Bacteroidetes abundance decreased in the EEN group. In the EEN group, significant changes in the ß-diversity of the microbiota were observed. In the analysis of microbiome species, abundances of Akkermansia muciniphila, Clostridium cocleatum, mucin-degrading bacteria, Flintibacter butyricus, and Parabacteroides goldsteinii, which are beneficial microbiota, were significantly increased in the EEN group compared to those in the NC group. More abundant mucins were confirmed in the colonic histopathology of the EEN group. These microbial and histopathological differences suggested that EEN might improve colitis symptoms in a murine colitis model by promoting mucin recycling and subsequently inducing the healing effect of the gut barrier. CONCLUSION: EEN showed clinical efficacy in a murine model of colitis. Based on the increase in mucin-degrading bacteria and the pathological increase in mucin production after EEN administration, it can be observed that mucin plays an important role in the therapeutic effect of EEN.
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Colite , Doença de Crohn , Microbioma Gastrointestinal , Animais , Colite/induzido quimicamente , Colite/patologia , Colite/terapia , Modelos Animais de Doenças , Humanos , Camundongos , Camundongos Endogâmicos C57BLRESUMO
BACKGROUND: Accurate and timely assessment of children's developmental status is crucial for early diagnosis and intervention. More accurate and automated developmental assessments are essential due to the lack of trained health care providers and imprecise parental reporting. In various areas of development, gross motor development in toddlers is known to be predictive of subsequent childhood developments. OBJECTIVE: The purpose of this study was to develop a model to assess gross motor behavior and integrate the results to determine the overall gross motor status of toddlers. This study also aimed to identify behaviors that are important in the assessment of overall gross motor skills and detect critical moments and important body parts for the assessment of each behavior. METHODS: We used behavioral videos of toddlers aged 18-35 months. To assess gross motor development, we selected 4 behaviors (climb up the stairs, go down the stairs, throw the ball, and stand on 1 foot) that have been validated with the Korean Developmental Screening Test for Infants and Children. In the child behavior videos, we estimated each child's position as a bounding box and extracted human keypoints within the box. In the first stage, the videos with the extracted human keypoints of each behavior were evaluated separately using a graph convolutional networks (GCN)-based algorithm. The probability values obtained for each label in the first-stage model were used as input for the second-stage model, the extreme gradient boosting (XGBoost) algorithm, to predict the overall gross motor status. For interpretability, we used gradient-weighted class activation mapping (Grad-CAM) to identify important moments and relevant body parts during the movements. The Shapley additive explanations method was used for the assessment of variable importance, to determine the movements that contributed the most to the overall developmental assessment. RESULTS: Behavioral videos of 4 gross motor skills were collected from 147 children, resulting in a total of 2395 videos. The stage-1 GCN model to evaluate each behavior had an area under the receiver operating characteristic curve (AUROC) of 0.79 to 0.90. Keypoint-mapping Grad-CAM visualization identified important moments in each behavior and differences in important body parts. The stage-2 XGBoost model to assess the overall gross motor status had an AUROC of 0.90. Among the 4 behaviors, "go down the stairs" contributed the most to the overall developmental assessment. CONCLUSIONS: Using movement videos of toddlers aged 18-35 months, we developed objective and automated models to evaluate each behavior and assess each child's overall gross motor performance. We identified the important behaviors for assessing gross motor performance and developed methods to recognize important moments and body parts while evaluating gross motor performance.
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Although recent dramatic advances in power conversion efficiencies (PCEs) have resulted in values over 19%, the poor photostability of organic photovoltaics (OPVs) has been a serious bottleneck to their commercialization. The photocatalytic effect, which is caused by incident ultraviolet-A (UV-A, 320-400 nm) light in the most commonly used zinc oxide (ZnOX) electron transport layer (ETL), significantly deteriorates the photostability of OPVs. In this work, we develop a new and facile method to enhance the photostability of nonfullerene acceptor-based OPVs by introducing UV-A-insensitive titanium suboxide (TiOX) ETL. Through an in-depth analysis of mass information at the interface between the ETL and photoactive layer, we confirm that the UV-A-insensitive TiOX suppresses the photocatalytic effect. The resulting device employing the TiOX ETL shows excellent photostability, obtaining 80% of the initial PCE for up to 200 h under 1 sun illumination, which is 10 times longer than that of the conventional ZnOX system (19 h).
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The development of an ideal solution-processable transparent electrode has been a challenge in the field of all-solution-processed semitransparent organic solar cells (ST-OSCs). We present a novel poly(3,4-ethylenedioxythiophene):polystyrenesulfonate (PEDOT:PSS) top electrode for all-solution-processed ST-OSCs through in situ doping of PEDOT:PSS. A strongly polarized long perfluoroalkyl (n = 8) chain-anchored sulfonic acid effectively eliminates insulating PSS and spontaneously crystallizes PEDOT at room temperature, leading to outstanding electrical properties and transparency of PEDOT top electrodes. Doped PEDOT-based ST-OSCs yield a high power conversion efficiency of 10.9% while providing an average visible transmittance of 26.0% in the visible range. Moreover, the strong infrared reflectivity of PEDOT enables ST-OSCs to reject 62.6% of the heat emitted by sunlight (76.7% from infrared radiation), outperforming the thermal insulation capability of commercial tint films. This light management approach using PEDOT enables ST-OSCs to simultaneously provide energy generation and energy savings, making it the first discovery toward sustainable energy in buildings.
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Sepsis is a dysregulated immune response to infection that leads to organ dysfunction and is associated with a high incidence and mortality rate. The lack of reliable biomarkers for diagnosing and prognosis of sepsis is a major challenge in its management. We aimed to investigate the potential of three-dimensional label-free CD8 + T cell morphology as a biomarker for sepsis. This study included three-time points in the sepsis recovery cohort (N = 8) and healthy controls (N = 20). Morphological features and spatial distribution within cells were compared among the patients' statuses. We developed a deep learning model to predict the diagnosis and prognosis of sepsis using the internal cell morphology. Correlation between the morphological features and clinical indices were analysed. Cell morphological features and spatial distribution differed significantly between patients with sepsis and healthy controls and between the survival and non-survival groups. The model for predicting the diagnosis and prognosis of sepsis showed an area under the receiver operating characteristic curve of nearly 100% with only a few cells, and a strong correlation between the morphological features and clinical indices was observed. Our study highlights the potential of three-dimensional label-free CD8 + T cell morphology as a promising biomarker for sepsis. This approach is rapid, requires a minimum amount of blood samples, and has the potential to provide valuable information for the early diagnosis and prognosis of sepsis.
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The study of quantum phase transitions that are not clearly associated with broken symmetry is a major effort in condensed matter physics, particularly in regard to the problem of high-temperature superconductivity, for which such transitions are thought to underlie the mechanism of superconductivity itself. Here we argue that the putative quantum critical point in the prototypical unconventional superconductor CeCoIn5 is characterized by the delocalization of electrons in a transition that connects two Fermi surfaces of different volumes, with no apparent broken symmetry. Drawing on established theory of f-electron metals, we discuss an interpretation for such a transition that involves the fractionalization of spin and charge, a model that effectively describes the anomalous transport behavior we measured for the Hall effect.
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The advent of special types of polymeric semiconductors, known as "polymer blends," presents new opportunities for the development of next-generation electronics based on these semiconductors' versatile functionalities in device applications. Although these polymer blends contain semiconducting polymers (SPs) mixed with a considerably high content of insulating polymers, few of these blends unexpectedly yield much higher charge carrier mobilities than those of pure SPs. However, the origin of such an enhancement has remained unclear owing to a lack of cases exhibiting definite improvements in charge carrier mobility, and the limited knowledge concerning the underlying mechanism thereof. In this study, the morphological changes and internal nanostructures of polymer blends based on various SP types with different intermolecular interactions in an insulating polystyrene matrix are investigated. Through this investigation, the physical confinement of donor-acceptor type SP chains in a continuous nanoscale network structure surrounded by polystyrenes is shown to induce structural ordering with more straight edge-on stacked SP chains. Hereby, high-performance and transparent organic field-effect transistors with a hole mobility of ≈5.4 cm2 V-1 s-1 and an average transmittance exceeding 72% in the visible range are achieved.
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We fabricated window-film-type organic photovoltaics with flexible transparent electrodes (FTEs). By overcoming the poor adhesion between layers, we created ultrathin metal electrodes (bottom FTE) on flexible substrates and transferred conducting polymers onto the photoactive layer (top FTE), providing power conversion efficiencies of 4.9% (7.4%) with average visible transmittances of 38% (18%).
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Organic photosensitizers have been investigated as effective light-sensing elements that can promote strong absorption with high field-effect mobility in organic phototransistors (OPTs). In this study, a novel organic photosensitizer is synthesized to demonstrate broad-band photoresponse with enhanced electrical performance. An unsymmetrical small molecule of a solubilizing donor (Dsol)-acceptor (A)-dye donor (Ddye) type connected with a twisted conjugation system is designed for broad-band detection (ranging from 250 to 700 nm). This molecule has high solubility, thereby facilitating the formation of uniformly dispersed nanoparticles in an insulating polymer matrix, which is deposited on top of OPT semiconductors by a simple solution process. The broad-band photodetection shown by the organic photosensitizer is realized with improved mobility close to an order of magnitude and high on/off current ratio (â¼105) of the organic semiconductor. Furthermore, p-type charge transport behavior in the channel of the OPT is enhanced through the intrinsic electron-accepting ability of the organic photosensitizer caused by the unique molecular configuration. These structural properties of organic photosensitizers contribute to an improvement in broad-band photosensing systems with new optoelectronic properties and functionalities.
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Our understanding of correlated electron systems is vexed by the complexity of their interactions. Heavy fermion compounds are archetypal examples of this physics, leading to exotic properties that weave magnetism, superconductivity and strange metal behavior together. The Kondo semimetal CeSb is an unusual example where different channels of interaction not only coexist, but have coincident physical signatures, leading to decades of debate about the microscopic picture describing the interactions between the f moments and the itinerant electron sea. Using angle-resolved photoemission spectroscopy, we resonantly enhance the response of the Ce f electrons across the magnetic transitions of CeSb and find there are two distinct modes of interaction that are simultaneously active, but on different kinds of carriers. This study reveals how correlated systems can reconcile the coexistence of different modes on interaction-by separating their action in momentum space, they allow their coexistence in real space.
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The synthesis of a diseleno[3,2-b:2',3'-d]selenophene (DSS) composed of three fused selenophenes is reported and it is used as a building block for the preparation of a high hole mobility conjugated polymer (PDSSTV). The polymer demonstrates strong intermolecular interactions even in solution, despite steric repulsion between the large Se atom in DSS and adjacent (Cß)-H atoms which leads to a partially twisted confirmation PDSSTV. Nevertheless, 2D grazing incidence X-ray diffraction (2D-GIXD) analysis reveals that the polymer tends to align in a highly ordered edge-on orientation after thermal annealing. The polymer demonstrates promising performance in a field-effect transistor device with saturated hole mobility up to 2 cm2 V-1 s-1 obtained under relatively low gate voltages of -30 V. The ultilization of a Se-containing fused aromatic system, therefore, appears to be a promising avenue for the development of high-performance conjugated polymers.
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[This corrects the article DOI: 10.1002/advs.201900245.].
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We analyse organic solar cells with four different photoactive blends exhibiting differing dependencies of short-circuit current upon photoactive layer thickness. These blends and devices are analysed by transient optoelectronic techniques of carrier kinetics and densities, air photoemission spectroscopy of material energetics, Kelvin probe measurements of work function, Mott-Schottky analyses of apparent doping density and by device modelling. We conclude that, for the device series studied, the photocurrent loss with thick active layers is primarily associated with the accumulation of photo-generated charge carriers in intra-bandgap tail states. This charge accumulation screens the device internal electrical field, preventing efficient charge collection. Purification of one studied donor polymer is observed to reduce tail state distribution and density and increase the maximal photoactive thickness for efficient operation. Our work suggests that selecting organic photoactive layers with a narrow distribution of tail states is a key requirement for the fabrication of efficient, high photocurrent, thick organic solar cells.
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Despite the high expectation of deformable and see-through displays for future ubiquitous society, current light-emitting diodes (LEDs) fail to meet the desired mechanical and optical properties, mainly because of the fragile transparent conducting oxides and opaque metal electrodes. Here, by introducing a highly conductive nanofibrillated conducting polymer (CP) as both deformable transparent anode and cathode, ultraflexible and see-through polymer LEDs (PLEDs) are demonstrated. The CP-based PLEDs exhibit outstanding dual-side light-outcoupling performance with a high optical transmittance of 75% at a wavelength of 550 nm and with an excellent mechanical durability of 9% bending strain. Moreover, the CP-based PLEDs fabricated on 4 µm thick plastic foils with all-solution processing have extremely deformable and foldable light-emitting functionality. This approach is expected to open a new avenue for developing wearable and attachable transparent displays.
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Fluorine (F) substitution on conjugated polymers in polymer solar cells (PSCs) has a diverse effect on molecular properties and device performance. We present a series of three D-A type conjugated polymers (PBT, PFBT, and PDFBT) based on dithienothiophene and benzothiadiazole units with different numbers of F atoms to explain the influence of F substitution by comparing the molecular interactions of the polymers and the recombination kinetics in PSCs. The preaggregation behavior of PFBT and PDFBT in o-DCB at the UV-vis absorption spectra proves that both polymers have strong intermolecular interactions. Besides, more closely packed structures and change into face-on orientation of fluorinated polymers are observed in polymer:PC71BM blends by GIXD which is beneficial for charge transport and, ultimately, for current density in PSCs (4.3, 13.0, and 14.5 mA cm-2 for PBT, PFBT, and PDFBT, respectively). Also, the introduction of F atoms on conjugated backbones affects the recombination kinetics by suppressing bimolecular recombination, thereby improving the fill factor (0.41, 0.68, and 0.69 for PBT, PFBT, and PDFBT, respectively). Consequently, the PCE of PSCs reached 7.3% without any additional treatment (annealing, solvent additive, etc.) in the polymer containing difluorinated BT (PDFBT) that is much higher than nonfluorinated BT (PBT â¼ 1%) and monofluorinated BT (PFBT â¼ 6%).